This work incorporates ML complexes as unbound entities that interact with ML complexes bound to the backbone of the polymer. The pi-pi interactions and Coulombic forces between bound and unbound ML complexes hold the ML-rich phase together and result in improved mechanical properties over polymers containing only the bound ML complexes. The ML-rich phase formed ordered, cylindrical domains. The storage modulus, surface elastic modulus, and high temperature stability of these metallopolymers increased with increasing concentration of ML complex in the polymer while an optimal concentration and morphology are necessary to improve the strength and creep resistance of the polymer. Ultimately, the successful addition and patterning of unbound ML complexes as a hard phase in a polymer matrix provides an important template for the design of a new type of supramolecular nanocomposite.